WO2012114619A1 - Dispositif électroluminescent (el) organique - Google Patents

Dispositif électroluminescent (el) organique Download PDF

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Publication number
WO2012114619A1
WO2012114619A1 PCT/JP2011/079203 JP2011079203W WO2012114619A1 WO 2012114619 A1 WO2012114619 A1 WO 2012114619A1 JP 2011079203 W JP2011079203 W JP 2011079203W WO 2012114619 A1 WO2012114619 A1 WO 2012114619A1
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Prior art keywords
substrate
layer
organic
electrode
organic layer
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PCT/JP2011/079203
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English (en)
Japanese (ja)
Inventor
将啓 中村
正人 山名
山木　健之
大貴 加藤
貴裕 小柳
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パナソニック株式会社
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Priority to CN201180067770.2A priority Critical patent/CN103370985B/zh
Priority to US13/985,297 priority patent/US9461264B2/en
Publication of WO2012114619A1 publication Critical patent/WO2012114619A1/fr

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    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K50/00—Organic light-emitting devices
    • H10K50/80—Constructional details
    • H10K50/805—Electrodes
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05B—ELECTRIC HEATING; ELECTRIC LIGHT SOURCES NOT OTHERWISE PROVIDED FOR; CIRCUIT ARRANGEMENTS FOR ELECTRIC LIGHT SOURCES, IN GENERAL
    • H05B33/00—Electroluminescent light sources
    • H05B33/12—Light sources with substantially two-dimensional radiating surfaces
    • H05B33/26—Light sources with substantially two-dimensional radiating surfaces characterised by the composition or arrangement of the conductive material used as an electrode
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K50/00—Organic light-emitting devices
    • H10K50/80—Constructional details
    • H10K50/805—Electrodes
    • H10K50/81—Anodes
    • H10K50/813—Anodes characterised by their shape
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K71/00—Manufacture or treatment specially adapted for the organic devices covered by this subclass
    • H10K71/50—Forming devices by joining two substrates together, e.g. lamination techniques

Definitions

  • the present invention relates to an organic EL device in which an electrode extraction portion is formed.
  • An electroluminescence (EL) element is formed by forming a light emitting layer sandwiched between an anode and a cathode on a transparent substrate. When a voltage is applied between the electrodes, electrons and holes injected as carriers in the light emitting layer are formed. Light is emitted by excitons generated by recombination.
  • the EL elements are roughly classified into an organic EL element using an organic substance as a fluorescent material of a light emitting layer and an inorganic EL element using an inorganic substance.
  • the organic EL element can emit light with high luminance at a low voltage, and various emission colors can be obtained depending on the type of the fluorescent material, and it can be easily manufactured as a flat light-emitting panel. Used as a display device or a backlight. Furthermore, in recent years, a device corresponding to high luminance has been realized and attention has been paid to using it for a lighting fixture.
  • a transparent electrode such as ITO is formed on a glass substrate as an anode, and an organic layer including a light emitting layer made of an organic light emitting material is formed on the anode.
  • a metal thin film layer such as aluminum is formed as a cathode. Since the anode exists between the substrate and the organic layer, in order to connect the anode to the external power feeding terminal, a part of the anode or a part of the auxiliary electrode that assists the conductivity of the anode is formed in the organic layer. It extends outside the region, and this extended portion functions as an electrode extraction portion.
  • the anode, the organic layer, and the cathode are sealed with a sealing member such as a copper foil except for the extraction electrode portion of the anode and a part of the cathode.
  • a voltage applied between the anode and the cathode and light generated in the light emitting layer is reflected directly or by the cathode, passes through the anode and the glass substrate, and is taken out of the device.
  • the organic layer including the light-emitting layer of the organic EL element is made of an organic material such as a polymer. It can have. Some of these organic materials can form a light emitting layer by vacuum coating, spin coating, ink jet printing, screen printing, or the like. Further, the substrate is not limited to the glass substrate described above, and a light-transmitting plastic substrate having flexibility can also be used. By using these materials, the organic EL element can be used as a light source of a flexible light-emitting device that can be wound and bent.
  • a so-called roll-to-roll system in which a flexible substrate wound in a roll shape is supplied to a film forming apparatus to form a light emitting layer and the like, and a device after film formation is wound in a roll shape and collected.
  • a method of manufacturing an organic EL device is known (for example, see Japanese Patent Application Laid-Open No. 2010-165620 published in Japanese Patent Application).
  • Patent Document 1 does not specifically describe how to form the electrode extraction portion. Usually, in order to provide an electrode extraction part, it is necessary to pattern the anode and the light-emitting layer in a complicated shape. Even in the manufacturing method using the roll-to-roll method described above, the device is not necessarily manufactured efficiently. I could not.
  • the present invention has been made in view of the above problems, and an object of the present invention is to provide an organic EL device that can easily form an electrode extraction portion and can be efficiently manufactured.
  • an organic EL device includes a first substrate having conductivity, an organic layer formed on the first substrate, and a second substrate having translucency.
  • An electrode layer formed on the second substrate, and the surface of the first substrate on which the organic layer is formed and the surface of the second substrate on which the electrode layer is formed face each other.
  • the organic layer is not formed in any region of the peripheral portion of the second substrate, and the second substrate is disposed in a portion facing the region where the organic layer is not formed.
  • a part of the electrode layer is extended to the outer peripheral side from a region where the organic layer is present, and the first substrate does not exist in a portion facing the extended electrode layer, and extends.
  • the electrode layer exposed from the first substrate constitutes an electrode extraction portion.
  • the first substrate and the second substrate are bonded by an adhesive layer provided on a peripheral portion of the first substrate or the second substrate.
  • a moisture absorbing layer is formed on a surface of the second substrate facing the electrode layer so as not to overlap with a region where the organic layer is formed and so as not to contact the electrode layer. Is preferably provided.
  • the electrode take-out part is preferably sealed with a sealing material except for a part of the electrode layer.
  • a part of the sealing material is a member in which the adhesive layer is extended.
  • the sealing material is preferably a separate member from the adhesive layer.
  • the electrode layer is preferably composed of a main electrode portion that is in contact with the organic layer, and an auxiliary electrode portion that is in contact with the main electrode portion and insulated from the organic layer. .
  • the electrode layer of the electrode extraction part is preferably a part of the auxiliary electrode part.
  • the main electrode portion is preferably composed of a grid electrode in which thin wires having low resistance are arranged in a lattice shape, a line shape, or a honeycomb shape.
  • the first substrate is preferably made of a metal material having a barrier property.
  • the electrode layer extending in the region where the organic layer is not formed is exposed from the first substrate and becomes an electrode extraction portion, it is easy to remove the first substrate, etc.
  • the electrode extraction part can be formed by a simple procedure, and the organic EL device can be manufactured efficiently.
  • FIG. 1 is an exploded perspective view of an organic EL device according to an embodiment of the present invention.
  • the back view of the organic EL device (A) is a side sectional view taken along line (A) or (D) in FIG. 2, (b) is a side sectional view taken along line (B) in FIG. 2, and (c) is a line (C) in FIG. FIG.
  • the perspective view of the electrode extraction part of the organic EL device The perspective view which shows the structural example of the grid electrode used as an electrode layer of the organic EL device.
  • or (e) is a sectional side view which shows the preparation procedures of the electrode extraction part of the organic EL device.
  • the organic EL device 1 includes a first substrate 2 having conductivity, an organic layer 3 formed on the first substrate 2, and a second light-transmitting material.
  • the substrate 6 and the electrode layer 4 formed on the second substrate 6 are provided.
  • the surface of the first substrate 2 on which the organic layer 3 is formed and the surface of the second substrate 6 on which the electrode layer 4 is formed are arranged in contact with each other.
  • the first substrate 2 not only functions as a substrate for forming the organic layer 3 but also functions as a cathode that supplies electrons.
  • the electrode layer 4 functions as an anode that supplies holes to the organic layer 3.
  • the organic layer 3 includes an electron injection layer 31, a light emitting layer 32, a hole transport layer 33, and a hole injection layer 34 in this order from the first substrate 2 side.
  • the electrode layer 4 includes a main electrode portion 41 that is in contact with the organic layer 3 and an auxiliary electrode portion 42 that is in contact with the main electrode portion 41 and is insulated from the organic layer 3 by the insulating layer 7.
  • the adhesive layer 5 includes a moisture absorption layer 8, and the moisture absorption layer 8 is sandwiched between the first substrate 2 and the second substrate 6 so as to be located on the outer periphery of the insulating layer 7.
  • the organic layer 3 is not formed in any region on the peripheral edge of the second substrate 6.
  • the organic layer 3 is not formed in the portions indicated by the lines (B) and (C) in FIG.
  • the region where the organic layer 3 is not formed may be provided on any one of the four sides of the second substrate 6, and may not be provided over the entire length of one side. It may be provided (not shown).
  • the organic layer 3 is formed up to the end portions in the portions indicated by the lines (A) and (D) in FIG. 2 (see also FIG. 3A).
  • the roll traveling direction is the line (A) in FIG.
  • a holding member (not shown) that seals the organic layer 3 and the like and protects the side portion of the organic EL device 1 is provided on both sides including the portions indicated by the lines (A) and (D) in FIG. .
  • This holding member may be provided on both sides including the portions indicated by the lines (B) and (C) in FIG.
  • auxiliary electrode portion 42 extends through the insulating layer 7. (See FIG. 1).
  • the extended auxiliary electrode portion 42 constitutes an electrode extraction portion 40 by exposing the opposing first substrate 2 to be removed.
  • a part of the exposed auxiliary electrode portion 42 is electrically connected to an external power feeding terminal or the like.
  • the formation procedure of the electrode extraction part 40 is mentioned later.
  • a sheet material made of a metal or an alloy such as aluminum, copper, stainless steel, nickel, tin, lead, gold, silver, iron or titanium is used, and the sheet material can be rolled up. Those having a certain degree of flexibility are preferred.
  • the surface of the sheet material needs to have smoothness in order to suppress a short circuit of the element, and the surface roughness is preferably Ra 100 nm or less, and more preferably Ra 10 nm or less.
  • the first substrate 2 is preferably made of a metal material having a barrier property against moisture, gas, and the like. By so doing, it is possible to suppress deterioration of the organic layer 3 due to moisture, gas, or the like. Moreover, since the 1st board
  • a metal such as aluminum or silver, or a compound containing these metals can be used, and a layered structure or the like formed by combining aluminum and another electrode material is used.
  • Examples of such electrode material combinations include a laminate of an alkali metal and aluminum, a laminate of an alkali metal and silver, a laminate of an alkali metal halide and aluminum, and a laminate of an alkali metal oxide and aluminum.
  • the electron injection layer 31 constituting the organic layer 3 includes the same material as that constituting the first substrate 2, a metal oxide such as titanium oxide and zinc oxide, and a dopant that promotes electron injection, including the above materials.
  • An organic semiconductor material mixed with or the like is used.
  • the light emitting layer 32 any material known as a light emitting material of the organic EL element is used.
  • luminescent materials include anthracene, naphthalene, pyrene, tetracene, coronene, perylene, phthaloperylene, naphthaloperylene, diphenylbutadiene, tetraphenylbutadiene, coumarin, oxadiazole, bisbenzoxazoline, bisstyryl, cyclopentadiene, quinoline.
  • Metal complex tris (8-hydroxyquinolinato) aluminum complex, tris (4-methyl-8-quinolinato) aluminum complex, tris (5-phenyl-8-quinolinato) aluminum complex, aminoquinoline metal complex, benzoquinoline metal complex , Tri- (p-terphenyl-4-yl) amine, pyran, quinacridone, rubrene, and derivatives thereof, or 1-aryl-2,5-di (2-thienyl) pyrrole derivatives, di Chirirubenzen derivatives, styryl arylene derivatives, styrylamine derivatives, and compounds or polymers such having a group consisting of these luminescent compound in a portion of the molecule.
  • phosphorescent materials for example, luminescent materials such as Ir complexes, Os complexes, Pt complexes, and europium complexes, or compounds having these in the molecule, or Polymers can also be suitably used.
  • the light emitting layer 32 made of these materials may be formed by a dry process such as vapor deposition or transfer, or may be formed by application such as spin coating, spray coating, die coating, or gravure printing. .
  • the hole transport layer 33 can be selected from a group of compounds having hole transport properties, for example.
  • this type of compound include 4,4′-bis [N- (naphthyl) -N-phenyl-amino] biphenyl ( ⁇ -NPD), N, N′-bis (3-methylphenyl)-(1 , 1′-biphenyl) -4,4′-diamine (TPD), 2-TNATA, 4,4 ′, 4 ′′ -tris (N- (3-methylphenyl) N-phenylamino) triphenylamine (MTDATA) 4,4'-N, N'-dicarbazole biphenyl (CBP), spiro-NPD, spiro-TPD, spiro-TAD, TNB, and the like, triarylamine compounds, amine compounds containing carbazole groups , Amine compounds containing a fluorene derivative, and the like, and any generally known hole transport material can be used.
  • Examples include low molecular weight organic compounds such as talocyanine (CuPc), and organic materials including thiophene triphenylmethane, hydrazoline, arylamine, hydrazone, stilbene, triphenylamine, etc.
  • organic materials including thiophene triphenylmethane, hydrazoline, arylamine, hydrazone, stilbene, triphenylamine, etc.
  • PVCz polyvinylcarbazole
  • PEDOT Polystyrene sulfonate
  • aromatic amine derivatives such as TPD, etc.
  • any material known as an anode material of an organic EL element can be used.
  • Anode materials include silver, indium-tin oxide (ITO), indium-zinc oxide (IZO), tin oxide, nanowires of metals such as gold, nanoparticles containing nanodots, conductive polymers, conductive Organic material, dopant (donor or acceptor) -containing organic layer, and a mixture of a conductor and a conductive organic material (including a polymer), as long as it has conductivity and translucency, but is not limited thereto. .
  • a binder may be included in addition to the conductive substance.
  • Binders include acrylic resin, polyethylene, polypropylene, polyethylene terephthalate, polymethyl methacrylate, polystyrene, polyethersulfone, polyarylate, polycarbonate resin, polyurethane, polyacrylonitrile, polyvinyl acetal, polyamide, polyimide, diacrylphthalate resin, and cellulose.
  • Examples thereof include resins, polyvinyl chloride, polyvinylidene chloride, polyvinyl acetate, other thermoplastic resins, and two or more copolymers of monomers constituting these resins.
  • the main electrode portion 41 may be composed of a so-called grid electrode 41 ′ in which thin wires 43 having low resistance are arranged in a lattice shape, a line shape, or a honeycomb shape. Good.
  • the diameter of the fine wire 43 is preferably 100 ⁇ m or less so that the translucency of the main electrode portion 41 is hardly lowered.
  • the interval between the thin wire members 43 is set wide as long as the conductivity can be maintained, and preferably the aperture ratio is 90% or more. Is set as follows.
  • Examples of the thin wire 43 include various metals and alloys such as silver, aluminum, copper, nickel, tin, lead, gold, and titanium, and conductive materials such as carbon.
  • the grid electrode 41 ′ is formed by patterning the paste containing the metal or the conductive material on the organic layer 3 by screen printing, gravure coating, die coating or the like.
  • the grid electrode 41 ′ is easy to form a film by coating, and is effective in efficiently manufacturing the organic EL device 1. These materials and forming methods are not particularly limited as long as they do not cause wettability to the organic layer 3 or damage to the organic layer 3.
  • the auxiliary electrode portion 42 is arranged in a frame shape so as to surround the periphery of the opposing organic layer 3, and a part of the auxiliary electrode portion 42 extends to the outer peripheral side from the region where the organic layer 3 is present as described above.
  • the provided part constitutes the electrode extraction part 40.
  • the auxiliary electrode portion 42 is formed by patterning on the second substrate 6 so as to have the shape described above, and the insulating layer 7 is disposed on the portion of the auxiliary electrode portion 42 that has a frame shape. That is, if a highly transparent material is used for the main electrode portion 41 facing the light emitting layer 32 and a highly conductive material is used for the surrounding auxiliary electrode portion 42, the electrode layer 4 as a whole has high translucency, In addition, the conductivity can be increased.
  • the constituent material of the auxiliary electrode part 42 is not particularly limited as long as various metals used for general wiring electrodes are used and the electrical conductivity with the main electrode part 41 is good. Further, unlike the main electrode portion 41, it does not have to
  • the adhesive layer 5 is disposed so that a paste-like or sheet-like member made of a resin material excellent in adhesiveness with the first substrate 2 and the insulating layer 7 covers the periphery of the organic layer 3 and the electrode layer 4.
  • a paste-like or sheet-like member made of a resin material excellent in adhesiveness with the first substrate 2 and the insulating layer 7 covers the periphery of the organic layer 3 and the electrode layer 4.
  • the constituent material of the adhesive layer 5 include silicone resin, fluororesin, acrylic resin, polyethylene, polypropylene, polyethylene terephthalate, polymethyl methacrylate, polystyrene, and polyvinyl acetate.
  • the second substrate 6 is a transparent plate-like member formed in the same shape as the first substrate 2, and has a uniform plate thickness and surface smoothness.
  • translucent glass such as soda lime glass or non-alkali glass, translucent resin material, or the like is used.
  • the insulating layer 7 is formed in a pattern so as to be substantially similar to the frame-like portion of the auxiliary electrode portion 42 and wider than the auxiliary electrode portion 42.
  • the insulating layer 7 is patterned so that the inner periphery thereof is larger than the outer periphery of the organic layer 3, thereby ensuring insulation between the auxiliary electrode portion 42 and the organic layer 3.
  • a thermosetting resin made of a thermosetting polyimide resin, an epoxy resin, or the like, or a thermoplastic resin such as polyethylene or polypropylene is formed by a wet process, or an oxidation such as silicon oxide or silicon nitride. And nitride can be formed by a dry process such as sputtering.
  • the insulating layer 7 can be formed preferably by a method such as screen printing, die coating, spray coating, or gravure coating. Note that the adhesive layer 5 can be replaced with the insulating layer 7 depending on the type, shape, and the like. In this case, the insulating layer 7 may not be provided.
  • the moisture absorbing layer 8 is formed by patterning a resin material containing a desiccant into a frame shape so that a region where the organic layer 3 is formed is opened. By providing the moisture absorbing layer 8, moisture that has slightly entered the adhesive layer 5 is blocked, so that deterioration of the organic layer 3 can be effectively suppressed.
  • the constituent material of the moisture absorption layer 8 is, for example, a photo-curing adhesive resin made of epoxy resin, acrylic resin, silicone resin, etc., calcium oxide, barium oxide, sodium oxide, potassium oxide, sodium sulfate, calcium sulfate. , Magnesium sulfate, calcium chloride, magnesium chloride, copper chloride, magnesium oxide and the like added with a desiccant can be used.
  • the moisture absorption layer 8 faces the 1st board
  • an organic layer 3 is laminated as shown in FIG.
  • the auxiliary electrode portion 42, the main electrode portion 41, and the insulating layer 7 are each patterned in a predetermined shape.
  • the first substrate 2 and the second substrate 6 are arranged so that the organic layer 3 and the electrode layer 4 (main electrode portion 41) are in contact with each other, and the second substrate.
  • a moisture absorbing layer 8 is provided at a predetermined position 6, and these are bonded and fixed by the adhesive layer 5 as shown in FIG. 6 (d).
  • the adhesive layer 5 is disposed so as not to cover the extended auxiliary electrode portion 42.
  • the auxiliary electrode portion 42 and the insulating layer 7 are configured in a frame shape (see FIG. 1), and the auxiliary electrode portion 42 and the insulating layer 7 are laminated so as to be thicker than the other portions. It functions as a dam that blocks the inflow to the layer 3 side.
  • the first substrate 2 facing the extended auxiliary electrode portion 42 is removed, and the auxiliary electrode portion 42 is exposed, whereby the electrode extraction portion 40 is formed.
  • the first substrate 2 and the second substrate 6 may be bonded after the first substrate 2 facing the extended auxiliary electrode portion 42 is removed.
  • the organic EL device 1 removes the first substrate 2 because the electrode layer 4 extending in a region where the organic layer 3 is not formed is exposed from the first substrate 2 and becomes the electrode extraction portion 40.
  • the electrode extraction part 40 can be formed by a simple procedure such as, and can be manufactured efficiently.
  • substrate 2, the organic layer 3, the insulating layer 7, the auxiliary electrode part 42, and the main electrode part 41 can use a flexible material, and can also use the 2nd board
  • the organic layer having the same configuration Both the flexible type and the hard type organic EL device 1 can be manufactured using the first substrate 6 with 3 attached.
  • the organic EL device 1 of the present embodiment can also use a strip-shaped sheet material supplied in a rolled state as the first substrate 2.
  • the organic layer 3 is continuously formed on the surface of the belt-shaped first substrate 2 by a slit coater or the like, and after the formation, it is wound up and collected again in a roll shape.
  • the sheet roll (not shown) which consists of the 1st board
  • the first substrate 2 is removed to form the electrode extraction portion 40.
  • the organic layer 3 tends to be multi-layered, such as the multilayering of the light emitting layer 32 and the arrangement of the charge adjustment layer therebetween, and the formation of the organic layer 3 by the roll-to-roll method is as follows. Many organic layers composed of multiple layers as described above can be produced simultaneously.
  • the present invention there is a region where the organic layer is not formed on the peripheral portion of the substrate, and a part of the substrate facing the electrode layer disposed in this region is removed to expose the electrode layer, whereby the electrode
  • the present invention is not limited to the above embodiment, and various modifications can be made.
  • Organic EL device First substrate (cathode) 3 Organic layer 4 Electrode layer (anode) DESCRIPTION OF SYMBOLS 40 Electrode extraction part 41 Main electrode part 42 Auxiliary electrode part 5 Adhesion layer 6 2nd board

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  • Engineering & Computer Science (AREA)
  • Manufacturing & Machinery (AREA)
  • Electroluminescent Light Sources (AREA)

Abstract

L'invention concerne un dispositif électroluminescent (EL) organique (1) qui comporte un premier substrat (2) qui a une certaine conductivité, une couche organique (3) formée sur le premier substrat (2), un second substrat (6) qui est transparent, et une couche d'électrode (4) formée sur le second substrat (6). La couche d'électrode (4) du premier substrat (2) et la couche organique (3) du second substrat (6) sont disposées de façon à être en contact mutuel. La couche organique (3) n'est pas formée dans une certaine région de la partie périphérique du second substrat. Dans la région où la couche organique (3) n'est pas formée, s'étend une partie de la couche d'électrode (4) s'étend et le premier substrat (2) n'est pas présent pour être tourné vers la couche d'électrode étendue. Une partie de la couche d'électrode (4) est exposée et constitue une partie d'extraction d'électrode (40). La couche d'électrode étendue (4) dans la région où la couche organique (3) n'est pas formée est exposée à l'extérieur du premier substrat (2) et forme la partie d'extraction d'électrode (40) ; par conséquent, la partie d'extraction d'électrode (40) peut être formée par une procédure simple telle que l'élimination du premier substrat (2), et la fabrication peut être conduite de manière efficace.
PCT/JP2011/079203 2011-02-21 2011-12-16 Dispositif électroluminescent (el) organique WO2012114619A1 (fr)

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CN201180067770.2A CN103370985B (zh) 2011-02-21 2011-12-16 有机电致发光器件
US13/985,297 US9461264B2 (en) 2011-02-21 2011-12-16 Organic EL device and method of manufacturing organic EL device

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JP2011-035172 2011-02-21
JP2011035172A JP5842088B2 (ja) 2011-02-21 2011-02-21 有機ｅｌデバイス及び有機ｅｌデバイスの製造方法

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JP2012174472A (ja) 2012-09-10
JP5842088B2 (ja) 2016-01-13
US20130320324A1 (en) 2013-12-05

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